Electron Beam Probe Research Articles

Toward Electrochemical Studies on the Nanometer and Atomic Scales: Progress, Challenges, and Opportunities.

Electrochemical reactions and ionic transport underpin the operation of a broad range of devices and applications, from energy storage and conversion to information technologies, as well as biochemical processes, artificial muscles, and soft actuators. Understanding the mechanisms governing function of these applications requires probing local electrochemical phenomena on the relevant time and length scales. Here, we discuss the challenges and opportunities for extending electrochemical characterization probes to the nanometer and ultimately atomic scales, including challenges in down-scaling classical methods, the emergence of novel probes enabled by nanotechnology and based on emergent physics and chemistry of nanoscale systems, and the integration of local data into macroscopic models. Scanning probe microscopy (SPM) methods based on strain detection, potential detection, and hysteretic current measurements are discussed. We further compare SPM to electron beam probes and discuss the applicability of electron beam methods to probe local electrochemical behavior on the mesoscopic and atomic levels. Similar to a SPM tip, the electron beam can be used both for observing behavior and as an active electrode to induce reactions. We briefly discuss new challenges and opportunities for conducting fundamental scientific studies, matter patterning, and atomic manipulation arising in this context.

A Fuzzy Inference System for Unsupervised Deblurring of Motion Blur in Electron Beam Calibration

This paper presents a novel method of restoring the electron beam (EB) measurements that are degraded by linear motion blur. This is based on a fuzzy inference system (FIS) and Wiener inverse filter, together providing autonomy, reliability, flexibility, and real-time execution. This system is capable of restoring highly degraded signals without requiring the exact knowledge of EB probe size. The FIS is formed of three inputs, eight fuzzy rules, and one output. The FIS is responsible for monitoring the restoration results, grading their validity, and choosing the one that yields to a better grade. These grades are produced autonomously by analyzing results of a Wiener inverse filter. To benchmark the performance of the system, ground truth signals obtained using an 18 μm wire probe were compared with the restorations. Main aims are therefore: (a) Provide unsupervised deblurring for device independent EB measurement; (b) improve the reliability of the process; and (c) apply deblurring without knowing the probe size. These further facilitate the deployment and manufacturing of EB probes as well as facilitate accurate and probe-independent EB characterization. This paper’s findings also makes restoration of previously collected EB measurements easier where the probe sizes are not known nor recorded.

Conversion of a Patterned Organic Resist into a High Performance Inorganic Hard Mask for High Resolution Pattern Transfer.

Polyphthalaldehyde is a self-developing resist material for electron beam and thermal scanning probe lithography (t-SPL). Removing the resist in situ (during the lithography process itself) simplifies processing and enables direct pattern inspection, however, at the price of a low etch resistance of the resist. To convert the material into a etch resistant hard mask, we study the selective cyclic infiltration of trimethyl-aluminum (TMA)/water into polyphthalaldehyde. It is found that TMA diffuses homogeneously through the resist, leading to material expansion and formation of aluminum oxide concurrent to the exposure to water and the degradation of the polyphthalaldehyde polymer. The plasma etch resistance of the infiltrated resist is significantly improved, as well as its stability. Using a silicon substrate coated with 13 nm silicon nitride and 7 nm cross-linked polystyrene, high resolution polyphthalaldehyde patterning is performed using t-SPL. After TMA/H2O infiltration, it is demonstrated that pattern transfer into silicon can be achieved with good fidelity for structures as small as 10 nm, enabling >10× amplification and low surface roughness. The presented results demonstrate a simplified use of polyphthalaldehyde resist, targeting feature scales at nanometer range, and suggest that trimethyl-aluminum infiltration can be applied to other resist-based lithography techniques.

Solar type III radio burst time characteristics at LOFAR frequencies and the implications for electron beam transport

Context. Solar type III radio bursts contain a wealth of information about the dynamics of electron beams in the solar corona and the inner heliosphere; this information is currently unobtainable through other means. However, the motion of different regions of an electron beam (front, middle, and back) have never been systematically analysed before. Aims. We characterise the type III burst frequency-time evolution using the enhanced resolution of LOFAR (LOw Frequency ARray) in the frequency range 30–70 MHz and use this to probe electron beam dynamics. Methods. The rise, peak, and decay times with a ~0.2 MHz spectral resolution were defined for a collection of 31 type III bursts. The frequency evolution was used to ascertain the apparent velocities of the front, middle, and back of the type III sources, and the trends were interpreted using theoretical and numerical treatments. Results. The type III time profile was better approximated by an asymmetric Gaussian profile and not an exponential, as was used previously. Rise and decay times increased with decreasing frequency and showed a strong correlation. Durations were shorter than previously observed. Drift rates from the rise times were faster than from the decay times, corresponding to inferred mean electron beam speeds for the front, middle, and back of 0.2, 0.17, 0.15 c, respectively. Faster beam speeds correlate with shorter type III durations. We also find that the type III frequency bandwidth decreases as frequency decreases. Conclusions. The different speeds naturally explain the elongation of an electron beam in space as it propagates through the heliosphere. The expansion rate is proportional to the mean speed of the exciter; faster beams expand faster. Beam speeds are attributed to varying ensembles of electron energies at the front, middle, and back of the beam.

In situ atomic-level observation of the formation of platinum silicide at platinum-silicon oxide interfaces under electron irradiation

In situ atomic-level observation of the formation of Pt2Si at Pt/SiOx interface by electronic excitation under electron irradiation was performed by using scanning transmission electron microscopy. Scanning of an electron-beam probe stimulates silicide formation at the Pt/SiOx interface; the change in the Pt column corresponding to Pt2Si formation with a crystallographic orientation of (001)Pt//(001)Pt2Si and [110]Pt//[110]Pt2Si was observed in high-angle annular dark-field images.

First-principles study of magnetic order in graphene nanoflakes as spin logic devices

Scale effect and topological frustration can form magnetic order in the finite graphene structures (graphene nanoflakes (GNFs)). In this paper, the GNFs that can generate large net electron spin or electron spin antiferromagnetic coupling between local regions of net electron spins are classified reasonably. Representative special GNF configurations are proposed to be effectively used as fundamental logic gate devices for ultra-fast high density spintronics, and theoretically investigated by the first-principles electron structure calculations based on spin-polarized density functional theory. The first-principles calculations are performed by utilizing all-electron numerical-orbital scheme in the M11-L form of meta-GGA exchange-correlation functional. The energy spectrum of singly occupied states and the isodensity surface of total spin distribution indicate evidently that spin-single-state electrons are localized on two sides of a representative double-triangle GNF and the spin polarizations of two GNF segments are in opposite directions, resulting in antiferromagnetic coupling, which is consistent with the results derived from the graph theory and Lieb theorem. The energy of antiferromagnetic spin-coupled state is 55 meV lower than that of ferromagnetic spin-coupled state, which is obviously higher than the thermodynamic threshold of the minimum energy dissipation at room temperature. The spin coupling energy of the double triangle GNF increases with the scaling of GNF dimension increasing. The magnetic coupling strength of the double triangle GNF with and without mirror symmetry approach to the maximum stable values of 50 meV and 200 meV respectively, which are remarkably higher that of quantum dots and transition metal atom systems. Due to the fact that the spin coupling strength of the GNF logic gate spin device can reach 200 meV, it can operate normally at ambient temperature with an error rate of 0.001 which can be easily improved by an error correction technique. The calculation results demonstrate that the proposed GNF logic gate can finely operate at ambient temperature with significantly low and correctable error rate. Recent experimental studies show that graphene nanodevices on a scale of only a few nanometers can be successfully fabricated by etching technique of electron beam and scanning probe. Furthermore, the properties of GNF spin logic devices are not sensitive to intrinsic defects. The triangular GNF with n carbon rings has only (n+2)2-3 carbon atoms, while it can endure n-1 internal defects, thus persisting in non-bond states and local magnetic moments. It is suggested that the full spin logic gate devices based on GNF can be realized by using the current advanced nano-processing technology.

Beam distribution reconstruction simulation for electron beam probe

An electron beam probe (EBP) is a detector which makes use of a low-intensity and low-energy electron beam to measure the transverse profile, bunch shape, beam neutralization and beam wake field of an intense beam with small dimensions. While it can be applied to many aspects, we limit our analysis to beam distribution reconstruction. This kind of detector is almost non-interceptive for all of the beam and does not disturb the machine environment. In this paper, we present the theoretical aspects behind this technique for beam distribution measurement and some simulation results of the detector involved. First, a method to obtain a parallel electron beam is introduced and a simulation code is developed. An EBP as a profile monitor for dense beams is then simulated using the fast scan method for various target beam profiles, including KV distribution, waterbag distribution, parabolic distribution, Gaussian distribution and halo distribution. Profile reconstruction from the deflected electron beam trajectory is implemented and compared with the actual profile, and the expected agreement is achieved. Furthermore, as well as fast scan, a slow scan, i.e. step-by-step scan, is considered, which lowers the requirement for hardware, i.e. Radio Frequency deflector. We calculate the three-dimensional electric field of a Gaussian distribution and simulate the electron motion in this field. In addition, a fast scan along the target beam direction and slow scan across the beam are also presented, and can provide a measurement of longitudinal distribution as well as transverse profile simultaneously. As an example, simulation results for the China Accelerator Driven Sub-critical System (CADS) and High Intensity Heavy Ion Accelerator Facility (HIAF) are given. Finally, a potential system design for an EBP is described.

Scanning electron microscope line-profile analysis of less-than-10-nm patterns

Scanning electron microscopes (SEMs) are widely used in various fields and have contributed to advances in nanotechnology. To analyse SEM images, it is necessary to consider the size of the probe electron (PE) beam and the range of PE scattering inside the pattern because they affect edge sharpness in SEM images. As the feature size of the sample drops to less than 10 nm, their effects become even more noticeable. In this study, we utilized Monte-Carlo simulation to clarify the effects of the size of the PE beam and the range of PE scattering for patterns with a line width less than 10 nm. Using a reference pattern with a known cross-sectional shape, we determined the PE beam full-width at half maximum (FWHM) for the simulation by fitting the simulation line profile to the experimental one. The resultant simulation SEM images matched the experimental ones for various PE beam FWHM conditions at acceleration voltages of 500 to 2400 V, even though the pattern dimensions differed from those of the reference pattern. These results indicate that analysis using Monte-Carlo simulation is an effective approach to clarifying SEM image formation and that the optimum observation conditions for patterns with a line width even less than 10 nm can be explored using simulation.

Probing electron beam effects with chemoresistive nanosensors during in situ environmental transmission electron microscopy

We report in situ and ex situ fabrication approaches to construct p-type (CuO) and n-type (SnO2) metal oxide nanowire devices for operation inside an environmental transmission electron microscope (TEM). By taking advantage of their chemoresistive properties, the nanowire devices were employed as sensitive probes for detecting reactive species induced by the interactions of high-energy electrons with surrounding gas molecules, in particular, for the case of O2 gas pressures up to 20 mbar. In order to rationalize our experimental findings, a computational model based on the particle-in-cell method was implemented to calculate the spatial distributions of scattered electrons and ionized oxygen species in the environmental TEM. Our approach enables the a priori identification and qualitative measurement of undesirable beam effects, paving the way for future developments related to their mitigation.

Prospects for electron beam aberration correction using sculpted phase masks

Technological advances in fabrication methods allowed the microscopy community to take incremental steps towards perfecting the electron microscope, and magnetic lens design in particular. Still, state of the art aberration-corrected microscopes are yet 20–30 times shy of the theoretical electron diffraction limit. Moreover, these microscopes consume significant physical space and are very expensive. Here, we show how a thin, sculpted membrane is used as a phase-mask to induce specific aberrations into an electron beam probe in a standard high resolution TEM. In particular, we experimentally demonstrate beam splitting, two-fold astigmatism, three-fold astigmatism, and spherical aberration.

Femtosecond time-resolved MeV electron diffraction

We report the experimental demonstration of femtosecond electron diffraction using high-brightness MeV electron beams. High-quality, single-shot electron diffraction patterns for both polycrystalline aluminum and single-crystal 1T-TaS2 are obtained utilizing a 5 fC (∼3 × 104 electrons) pulse of electrons at 2.8 MeV. The high quality of the electron diffraction patterns confirms that electron beam has a normalized emittance of ∼50 nm rad. The transverse and longitudinal coherence length is ∼11 and ∼2.5 nm, respectively. The timing jitter between the pump laser and probe electron beam was found to be ∼100 fs (rms). The temporal resolution is demonstrated by observing the evolution of Bragg and superlattice peaks of 1T-TaS2 following an 800 nm optical pump and was found to be 130 fs. Our results demonstrate the advantages of MeV electrons, including large elastic differential scattering cross-section and access to high-order reflections, and the feasibility of ultimately realizing below 10 fs time-resolved electron diffraction.

Time-Resolved Visualization of Laser-Induced Heating of Gold with MeV Ultrafast Electron Diffraction

Time-resolved electron diffraction employing MeV electron beams is demonstrated experimentally at the center for ultrafast diffraction and microscopy of Shanghai Jiao Tong University. A high-quality diffraction pattern is recorded by a single shot of electron pulse. Synchronization between the pump laser and the probe electron beam is achieved through measurement of electron deflection caused by the laser-induced plasmas in a metal tip. We study the ultrafast structural dynamics of the gold lattice excited by a femtosecond laser through tracing the change of Bragg peaks intensity at different time delays. It is expected that the combination of MeV ultrashort electron beams and femtosecond laser pulses will open many new opportunities in the ultrafast and ultrasmall world.

Ultrafast coherent lattice and incoherent carrier dynamics in bismuth: time-domain results

The investigations of transient electronic processes and their influence on coherent lattice dynamics in Bi by different femtosecond spectroscopy methods are reviewed. The results of broadband optical, x-ray, and ultrashort electron beam probes in the study of coherent phonons and incoherent carrier dynamics are compared. Some coherent phonon peculiarities arising at high excitation are described. The difference between phonons of different symmetries and various generation mechanisms are discussed, highlighting their assignment to the decay of particular excited electronic states of bismuth. Data analysis revealed significant wavevector dependence of electron–hole and electron–phonon coupling strength along the Г–T direction of the Brillouin zone. Comparison of the coherent amplitude as a function of the pump photon wavelength from 400 to 2500 nm for two different in symmetry Eg and A1g phonon modes with respective spontaneous resonance Raman profiles revealed that their generation mechanisms are quite distinct. Displacive excitation, which is the main mechanism for the generation of coherent A1g phonons, cannot be reduced to the Raman scattering responsible for the generation of lower symmetry coherent lattice modes.

Direct imaging of p-n junction in core-shell GaN wires.

While core-shell wire-based devices offer a promising path toward improved optoelectronic applications, their development is hampered by the present uncertainty about essential semiconductor properties along the three-dimensional (3D) buried p-n junction. Thanks to a cross-sectional approach, scanning electron beam probing techniques were employed here to obtain a nanoscale spatially resolved analysis of GaN core-shell wire p-n junctions grown by catalyst-free metal-organic vapor phase epitaxy on GaN and Si substrates. Both electron beam induced current (EBIC) and secondary electron voltage constrast (VC) were demonstrated to delineate the radial and axial junction existing in the 3D structure. The Mg dopant activation process in p-GaN shell was dynamically controlled by the ebeam exposure conditions and visualized thanks to EBIC mapping. EBIC measurements were shown to yield local minority carrier/exciton diffusion lengths on the p-side (∼57 nm) and the n-side (∼15 nm) as well as depletion width in the range 40-50 nm. Under reverse bias conditions, VC imaging provided electrostatic potential maps in the vicinity of the 3D junction from which acceptor Na and donor Nd doping levels were locally determined to be Na = 3 × 10(18) cm(-3) and Nd = 3.5 × 10(18) cm(-3) in both the axial and the radial junction. Results from EBIC and VC are in good agreement. This nanoscale approach provides essential guidance to the further development of core-shell wire devices.

Effect of Magnetic Materials on the In-Vessel Magnetic Configuration in KSTAR

KSTAR has a nonlinear magnetic material, INCOLOY® alloy 908 (Incoloy), in toroidal field and poloidal field (PF) coil systems. The effect of Incoloy on the magnetic configuration for the plasma initiation was investigated with systematic magnetic field measurements, finite element model (FEM) calculations, and in situ measurements of the magnetic properties. The profile of the vertical field near the field-null center was measured with a vertically movable electron beam (e-beam) probe and Hall sensor arrays in addition to pickup coils in the vacuum vessel. The measured profiles of the additional fields from Incoloy in the PF coils are in good agreement with the FEM calculations. In a typical KSTAR startup configuration, the effect of Incoloy is significant. First, it degrades the connection length significantly due to an additional vertical field in the field-null region, and second, it changes the radial and vertical stabilities by modifying the radial gradient of the vertical field. Initial up-down asymmetry measurements of the vertical fields showed very small static error fields from the PF coils. Calculations suggest that the main sources of the measured downshift of the plasma column are asymmetric eddy currents in the cryostat.

Scattering of electrons by vacuum fluctuations of plasma waves

Interaction between a probe electron beam and longitudinal electromagnetic oscillations of the Fermi plasma in metals (plasmons) is investigated by the methods of quantum electrodynamics. The quantum description of plasmons allows one to construct a consistent theory of the scattering process and point out the applicability limits of the existing semiclassical theories. The quantum description of plasmons leads to the concept of electromagnetic vacuum of longitudinal waves, which is the subject of the present study. The vacuum of longitudinal waves significantly deforms the shape of plasma dielectric permittivity, thus leading to the broadening of Langmuir peaks of scattered electrons, which has so far resisted theoretical analysis. The presence of the electromagnetic vacuum of longitudinal plasma waves has a considerable effect on the integral scattering probability of electrons by plasmons.

Determination of fluctuations in local symmetry and measurement by convergent beam electron diffraction: applications to a relaxor-based ferroelectric crystal after thermal annealing

Single crystals of Pb(Mg1/3Nb2/3)O3–31%PbTiO3(PMN–31%PT) are known for their complex domain structures at the nanometre scale. While their average symmetry has been studied by X-ray, neutron and electron diffraction methods, there is little knowledge about variations in symmetry at the local scale. Here, direct evidence is provided for the volume dependence and spatial dependence of symmetry fluctuations by using quantitative convergent beam electron diffraction and energy dispersive X-ray spectroscopy. Fluctuations in symmetry were determined by using different electron beam probe sizes ranging from ∼2 to 25 nm from a crystal ∼62 nm thick. The symmetry of PMN–31%PT was found to increase linearly as the average volume increased, and the local symmetry fluctuated from one location to another at the nanoscale. Energy dispersive X-ray spectroscopy indicates that chemical fluctuations are significant when the probe size decreases to ∼2 nm. The symmetry fluctuation is attributed to locally varying composition-dependent ionic displacements and spontaneous polarization.

Site-Specific Growth of Au–Pd Alloy Horns on Au Nanorods: A Platform for Highly Sensitive Monitoring of Catalytic Reactions by Surface Enhancement Raman Spectroscopy

Surface-enhanced Raman scattering (SERS) is a highly sensitive probe for molecular detection. The aim of this study was to develop an efficient platform for investigating the kinetics of catalytic reactions with SERS. To achieve this, we synthesized a novel Au-Pd bimetallic nanostructure (HIF-AuNR@AuPd) through site-specific epitaxial growth of Au-Pd alloy horns as catalytic sites at the ends of Au nanorods. Using high-resolution electron microscopy and tomography, we successfully reconstructed the complex three-dimensional morphology of HIF-AuNR@AuPd and identified that the horns are bound with high-index {11l} (0.25 < l < 0.43) facets. With an electron beam probe, we visualized the distribution of surface plasmon over the HIF-AuNR@AuPd nanorods, finding that strong longitudinal surface plasmon resonance concentrated at the rod ends. This unique crystal morphology led to the coupling of high catalytic activity with a strong SERS effect at the rod ends, making HIF-AuNR@AuPd an excellent bifunctional platform for in situ monitoring of surface catalytic reactions. Using the hydrogenation of 4-nitrothiophenol as a model reaction, we demonstrated that its first-order reaction kinetics could be accurately determined from this platform. Moreover, we clearly identified the superior catalytic activity of the rod ends relative to that of the rod bodies, owing to the different SERS activities at the two positions. In comparison with other reported Au-Pd bimetallic nanostructures, HIF-AuNR@AuPd offered both higher catalytic activity and greater detection sensitivity.

Spin-polarized scanning electron microscopy

Spin-polarized scanning electron microscopy (spin-SEM) is a magnetic domain observation method. In spin-SEM, polarization of secondary electrons emitted from a sample in a scanning electron microscope is detected by a spin detector and used as a signal for forming an image. The characteristics of spin-SEM are detection of all three magnetization vector components, which leads to the detection of the magnetization vector direction, high spatial resolution of around 3 nm and applicability to samples with rough or even 3D surfaces. Spin-SEM combined with other imaging methods using an electron probe beam such as scanning Auger electron microscopy for imaging element distribution and electron backscattering diffraction microscopy for imaging crystal direction distribution provides additional information that is important to study the magnetism. Spin-SEM with these excellent characteristics has a broad range of applications from basic research to applied research and developments in various industries.

Determination of the thickness of a gold layer deposited onto silicon via reflected electron spectroscopy

The energy spectra of electrons reflected from a gold layer deposited onto a silicon substrate have been measured when the energy losses are comparable with the energy of a probe electron beam (5 keV) and the elastic energy losses correspond to an electron-beam energy of 14 keV. A subsequent theory for calculating the energy spectra of electrons and light ions reflected from a multilayer target, which is used to interpret the energy spectra measured in the wide range of energy losses, has been developed. It is found that the elastic scattering processes in the gold layer (the thickness of which is tens of monolayers) substantially affect formation of the energy spectra. The Au layer thicknesses calculated by means of the developed theory are compared with those determined from the spectra of elastically reflected electrons. The errors of the Au layer thickness measurements via the proposed method are discussed.